Freshwater scarcity is an escalating global challenge that necessitates innovative and sustainable water supply solutions. In this study, a novel gum Arabic-alginate-carboxylated carbon nanotubes (GAC) aerogel composite was developed for atmospheric water harvesting (AWH) across a broad range of relative humid conditions. The aerogel combines a biopolymeric double-network framework with hygroscopic CaCl₂ and LiCl salts, while carboxylated carbon nanotubes (CNTs–COOH) act as photothermal agents to enhance solar-driven desorption. The GAC aerogel achieved water sorption capacities of 7 g/g at 90 % RH and 1.2 g/g at 20 % RH (25 °C). Under simulated solar irradiation (0.8 SUN, 800 W/m 2 ), the aerogel exhibited an equilibrium surface temperature of 65 °C and released 94.7 % of captured water within 6 h. The material achieved stable performance over ten adsorption–desorption cycles (~3 cycles/day) without degradation. Structural and physicochemical analyses (FTIR, XRD, Raman, SEM, TGA, and UV–vis-NIR) confirmed the aerogel's chemical structure, macroporous morphology and photo absorption efficiency. These results establish GAC as a highly effective and sustainable sorbent for scalable atmospheric water generation, offering significant potential for deployment in arid and water-stressed regions. • A novel gum Arabic/alginate/ CNTs-COOH (GAC) aerogel composite was developed for efficient atmospheric water harvesting. • The GAC aerogel composite exhibited a water sorption capacity of 7 g/g at 90 % RH, and 1.2 g/g at 20 % RH. • Up to 94.7 % of the captured water is efficiently released under solar irradiation within 6 h. • Surface temperature of GAC aerogel reaches 65 °C under solar irradiation (0.8 SUN). • The GAC aerogel could be reused for 15 adsorption-desorption cycles and achieved three cycles per day.